We report the synthesis of conjugated polymer nanoparticles carrying stable luminescent radical units. These monodisperse conjugated radical nanoparticles can be tuned in their diameter over several hundred nanometers. They are stable in aqueous medium and highly luminescent in the red and near infrared spectrum, representing a powerful future tool for bioimaging. Moreover, the polymer nanoparticles exhibit paramagnetic properties, making them highly suitable for dual-mode optical and magnetic resonance imaging. In this study, we investigate their synthesis, optical and magnetic properties, and use quantum mechanical calculations to elucidate the effect of the conjugated polymer backbone and electron-withdrawing substituents on the electronic properties of the open-shell molecule in the polymer network of the particles.